Time-resolved plasmonics in designed nanostructures

A metal nanoparticle can be considered as consisting of a base of positive ion cores and a sea of free electrons. When the free electrons are displaced, for example, by an incident electric field, a restoring force acts on the electrons. The electrons may then oscillate back and forth until equilibrium is reached. This oscillation occurs at the natural frequency, or eigenfrequency, of the system. By matching the driving frequency with this frequency, the amplitude (the maximum electron displacement) can be made large - the system is in resonance. This resonance mode is a plasmon. The separation of charge on that small length scale will result in a large field in the vicinity of the nanoparticle. This large field, often oscillating at optical frequencies, on the spatial scale of nanometers, has many potential applications, such as high-resolution microscopy, photo-voltaics, light emission and coherent control. Because of the interest in manipulating light on the nanoscale, particles having their resonances in the optical domain are often used. The collective electron oscillation, when resonantly excited, therefore occurs on the femtosecond timescale. Due to this ultrashort timescale, the dynamics are difficult to follow in time. The spatial confinement of the oscillation to the nanometer scale makes it challenging to also image them. This thesis explores ways of studying the ultrafast dynamics of plasmons spatially and temporally, simultaneously. Two types of experiments are discussed. The first is autocorrelation experiments where the induced and enhanced field is autocorrelated with itself. For one of these experiments, bowtie nanoantennas were manufactured, using the focused ion beam technique. In the second kind of experiment an infrared laser pulse is used to excite the plasmon, and a short attosecond pulse probes it. The work described in this thesis deals with the fabrication of nanostructures and the implementation of attosecond pulse generation schemes suitable for this purpose

High-order harmonic generation using a high-repetition-rate turnkey laser

We generate high-order harmonics at high pulse repetition rates using a turnkey laser. High-order harmonics at 400 kHz are observed when argon is used as target gas. In neon we achieve generation of photons with energies exceeding 90 eV ($\sim$13 nm) at 20 kHz. We measure a photon flux of 4.4$\cdot10^{10}$ photons per second per harmonic in argon at 100 kHz. Many experiments employing high-order harmonics would benefit from higher repetition rates, and the user-friendly operation opens up for applications of coherent extreme ultra-violet pulses in new research areas

Carrier-envelope phase dependent high-order harmonic generation with a high-repetition rate OPCPA-system

We study high-order harmonic generation with a high-repetition rate (200 kHz), few-cycle, driving laser, based on optical parametric chirped pulse amplification. The system delivers carrier-envelope phase stable, 8 fs, 10 μJ pulses at a central wavelength of 890 nm. High-order harmonics, generated in a high-pressure Ar gas jet, exhibit a strong CEP-dependence over a large spectral range owing to excellent stability of the driving laser pulses. This range can be divided into three spectral regions with distinct CEP influence. The observed spectral interference structures are explained by an analytical model based upon multiple pulse interferences.Marie Curie Research Training Network ATTOFELEuropean Research CouncilKnut and Alice Wallenberg foundationSwedish Foundation for Strategic ResearchSwedish Research Counci

Multiple Scenario Generation of Subsurface Models:Consistent Integration of Information from Geophysical and Geological Data throuh Combination of Probabilistic Inverse Problem Theory and Geostatistics

Neutrinos with energies above 1017 eV are detectable with the Surface Detector Array of the Pierre Auger Observatory. The identification is efficiently performed for neutrinos of all flavors interacting in the atmosphere at large zenith angles, as well as for Earth-skimming \u3c4 neutrinos with nearly tangential trajectories relative to the Earth. No neutrino candidates were found in 3c 14.7 years of data taken up to 31 August 2018. This leads to restrictive upper bounds on their flux. The 90% C.L. single-flavor limit to the diffuse flux of ultra-high-energy neutrinos with an E\u3bd-2 spectrum in the energy range 1.0 7 1017 eV -2.5 7 1019 eV is E2 dN\u3bd/dE\u3bd < 4.4 7 10-9 GeV cm-2 s-1 sr-1, placing strong constraints on several models of neutrino production at EeV energies and on the properties of the sources of ultra-high-energy cosmic rays

Secondary electron imaging of nanostructures using Extreme Ultra-Violet attosecond pulse trains and Infra-Red femtosecond pulses

Surface electron dynamics unfold at time and length scales down to attoseconds and nanometres, making direct imaging with extreme spatiotemporal resolution highly desirable. However, this has turned out to be a major challenge even with the advent of reliable attosecond light sources. In this paper, photoelectrons from Ag nanowires and nanoparticles excited by extreme ultraviolet (XUV) attosecond pulse trains and infrared femtosecond pulses using a PhotoEmission Electron Microscope (PEEM) are imaged. In addition, the samples were investigated using Scanning Electron Microscopy (SEM) and synchrotron based X-ray photoelectron spectroscopy (XPS). To achieve contrast between the nanostructures and the substrate in the XUV images, three different substrate materials were investigated: Cr, ITO and Au. While plasmonic field enhancement can be observed on all three substrates, only on Au substrates do the Ag nanowires appear significantly brighter than the substrate in XUV-PEEM imaging. 3-photon photoemission imaging of plasmonic hot-spots was performed where the autocorrelation trace is observed in the interference signal between two femtosecond Infra-Red (IR) beams with sub-cycle precision. Finally, using Monte Carlo simulations, it is shown how the secondary electrons imaged in the XUV PEEM can potentially reveal information on the attosecond time scale from the near surface region of the nanostructures

Sub-cycle ionization dynamics revealed by trajectory resolved, elliptically-driven high-order harmonic generation

The sub-cycle dynamics of electrons driven by strong laser fields is central to the emerging field of attosecond science. We demonstrate how the dynamics can be probed through high-order harmonic generation, where different trajectories leading to the same harmonic order are initiated at different times, thereby probing different field strengths. We find large differences between the trajectories with respect to both their sensitivity to driving field ellipticity and resonant enhancement. To accurately describe the ellipticity dependence of the long trajectory harmonics we must include a sub-cycle change of the initial velocity distribution of the electron and its excursion time. The resonant enhancement is observed only for the long trajectory contribution of a particular harmonic when a window resonance in argon, which is off-resonant in the field-free case, is shifted into resonance due to a large dynamic Stark shift

Size and shape dependent few-cycle near-field dynamics of bowtie nanoantennas

Metal nanostructures can transfer electromagnetic energy from femtosecond laser pulses to the near-field down to spatial scales well below the optical diffraction limit. By combining few-femtosecond laser pulses with photoemission electron microscopy, we study the dynamics of the induced few-cycle near-field in individual bowtie nanoantennas. We investigate how the dynamics depend on antenna size and exact bowtie shape resulting from fabrication. Different dynamics are, as expected, measured for antennas of different sizes. However, we also detect comparable dynamics differences between individual antennas of similar size. With Finite-difference time-domain simulations we show that these dynamics differences between similarly sized antennas can be due to small lateral shape variations generally induced during the fabrication

Direct subwavelength imaging and control of near-field localization in individual silver nanocubes

We demonstrate the control of near-field localization within individual silver nanocubes through photoemission electron microscopy combined with broadband, few-cycle laser pulses. We find that the near-field is concentrated at the corners of the cubes, and that it can be efficiently localized to different individual corners depending on the polarization of the incoming light. The experimental results are confirmed by finite-difference time-domain simulations, which also provide an intuitive picture of polarization dependent near-field localization in nanocubes. (C) 2015 AIP Publishing LLC